An international intercomparison was organized by Working Group 7, Internal Dosimetry, of the European Radiation Dosimetry Group in collaboration with Working Group 6, Computational Dosimetry, for measurement and Monte Carlo simulation of 241Am in three skull phantoms. The main objectives of this combined exercise were (1) comparison of the results of counting efficiency in fixed positions over each head phantom using different germanium detector systems, (2) calculation of the activity of 241Am in the skulls, (3) comparison of Monte Carlo simulations with measurements (spectrum and counting efficiency), and (4) comparison of phantom performance. This initiative collected knowledge on equipment, detector arrangements, calibration procedures, and phantoms used around the world for in vivo monitoring of 241Am in exposed persons, as well as on the Monte Carlo skills and tools of participants. Three skull phantoms (BfS, USTUR, and CSR phantoms) were transported from Europe (10 laboratories) to North America (United States and Canada). The BfS skull was fabricated with real human bone artificially labeled with 241Am. The USTUR skull phantom was made from the US Transuranium and Uranium Registries whole-body donor (case 0102) who was contaminated due to an occupational intake of 241Am; one-half of the skull corresponds to real contaminated bone, the other half is real human bone from a noncontaminated person. Finally, the CSR phantom was fabricated as a simple hemisphere of equivalent bone and tissue material. The three phantoms differ in weight, size, and shape, which made them suitable for an efficiency study. Based on their own skull calibration, the participants calculated the activity in the three European Radiation Dosimetry Group head phantoms. The Monte Carlo intercomparison was organized in parallel with the measurement exercise using the voxel representations of the three physical phantoms; there were 16 participants. Three tasks were identified with increasing difficulty: (1) Monte Carlo simulation of the simple CSR hemisphere and the Helmholz Zentrum München high-purity germanium detector for calculating the counting efficiency for the 59.54 keV photons of 241Am, in established measurement geometry; (2) Monte Carlo simulation of particular measurement geometries using the BfS and USTUR voxel phantoms and the Helmholz Zentrum München high-purity germanium detector detector; and (3) application of Monte Carlo methodology to calculate the calibration factor of each participant for the detector system and counting geometry (single or multidetector arrangement) to be used for monitoring a person in each in vivo facility, using complex skull phantoms. The results of both exercises resulted in the conclusion that none of the three available head phantoms is appropriate as a reference phantom for the calibration of germanium detection systems for measuring 241Am in exposed adult persons. The main reasons for this are: (1) lack of homogeneous activity distribution in the bone material, or (2) inadequate shape/size for simulating an adult skull. Good agreement was found between Monte Carlo results and measurements, which supports Monte Carlo calibration of body counters as an alternative method when appropriate physical phantoms are not available and the detector and source are well known.